Abstract

Here, the scalable synthesis of low‐density 3D macroscopic structure of graphene oxide (GO) interconnected with polydimethylsiloxane (PDMS) is reported. A controlled amount of PDMS is infused into the freeze‐dried foam to result into a very rigid structure with improved mechanical properties, such as tensile plasticity and toughness. The PDMS wets the graphene oxide sheets and acts like glue between the 2D sheets. Molecular dynamics simulations are used to further elucidate the mechanisms of the interactions of graphene oxide layers with PDMS. The ability of using the interconnecting graphene oxide foam as an effective oil–water separator and stable insulating behavior to elevated temperatures are further demonstrated. The structural rigidity of the sample is also tested using laser impact and compared with GO foam.

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